First-principles Study on Electronic Structure and Optical Properties of S and Al Doped Monolayer g-C3N4
LIU Chenxi1, PANG Guowang1, PAN Duoqiao1, SHI Leiqian1, ZHANG Lili1,*, LEI Bocheng1,*, ZHAO Xucai1, HUANG Yineng1,2
1 Xinjiang Laboratory of Phase Transitions and Microstructures in Condensed Matter, College of Physical Science and Technology, Yili Normal University, Yining 835000, Xinjiang, China 2 National Laboratory of Solid State Microstructures, School of Physics, Nanjing University, Nanjing 210093, China
Abstract: The g-C3N4 is a typical polymer semiconductor material, which can complete the photocatalytic reaction with high requirements for semiconductors under visible light. The electronic structures and optical properties of monolayer g-C3N4, S doped g-C3N4, Al doped g-C3N4, and S-Al doped g-C3N4 systems were investigated using plane-wave density functional theory with ultra-soft pseudopotentials. The results showed that the impurity atoms are most likely to be doped into g-C3N4 system at the position of S doped gap I and Al doped N2. Compared with the monola-yer g-C3N4, the doped systems have lattice distortion and redshift phenomenon, which expands the light absorption range of the system. It can be inferred that S, Al doped can improve the photocatalytic performance of the g-C3N4 system. The photocatalytic performance of the S-Al co-doped system is the best, because the molecular orbital of the co-doped system have strong delocalization, which is beneficial to improve the mobility of carriers. And it can make the deep energy level introduced by single doping shallow, and reduce the appearance of recombination center on the impurity energy level. Therefore, S-Al co-doped system can be used as an effective means to improve the photocatalytic activity of g-C3N4.
通讯作者:
*张丽丽,于2020年获得南京大学博士学位,现为伊犁师范大学物理科学与技术学院副教授,主要从事玻璃化转变机制、金属氧化物电子结构的计算机模拟研究,已在Scientific Reports、International Journal of Modern Physics B、European Physical Journal E、Journal of Molecular Modeling、OPTIK等期刊上发表论文80余篇。suyi2046@sina.com 雷博程,2019年毕业于伊犁师范大学,获得理学硕士学位。现为伊犁师范大学物理科学与技术学院讲师,目前从事金属氧化物磁性及光催化性能领域的研究,发表论文10余篇。lbc0428@sina.com
刘晨曦, 庞国旺, 潘多桥, 史蕾倩, 张丽丽, 雷博程, 赵旭才, 黄以能. S和Al掺杂单层g-C3N4电子结构与光学性质的第一性原理研究[J]. 材料导报, 2023, 37(9): 21100044-6.
LIU Chenxi, PANG Guowang, PAN Duoqiao, SHI Leiqian, ZHANG Lili, LEI Bocheng, ZHAO Xucai, HUANG Yineng. First-principles Study on Electronic Structure and Optical Properties of S and Al Doped Monolayer g-C3N4. Materials Reports, 2023, 37(9): 21100044-6.
1 Cao S, Yu J. The Journal of Physical Chemistry Letters, 2014, 5(12), 2101. 2 Mao N, Gao X, Zhang C, et al. Dalton Transactions:an International Journal of Inorganic Chemistry, 2019, 48(39), 14864. 3 Fei X, Tan H, Cheng B, et al. Journal of Physical Chemistry, 2020, 37(6), 2010027. 4 Antil B, Kumar L, Ranjan R, et al. ACS Applied Energy Materials, 2021, 4(4), 3118. 5 Fu J, Xu Q, Low J, et al. Applied Catalysis B, Environmental, 2019, 243, 556. 6 Song Y, She X, Yi J, et al. Physica Status Solidi (A), 2017, 214(5), 1600704. 7 Fujishima A, Honda K. Nature, 1972, 238(5358), 37. 8 Na S, Seo S, Lee H. Catalysts, 2020, 10(6), 679. 9 Wang X, Maeda K, Thomas A, et al. Nature Materials, 2009, 8(1), 76. 10 Zhu B, Zhang L, Cheng B, et al. Chinese Journal of Catalysis, 2021, 42(1), 115. 11 Li H, Wu Y, Li L, et al. Applied Surface Science, 2018, 457, 735. 12 Tong T, Zhu B, Jiang C, et al. Applied Surface Science, 2018, 433, 1175. 13 Ye J, Liu J, An Y. Applied Surface Science, 2020, 501, 144262. 14 Liu X, Ma R, Zhuang L, et al. Critical Reviews in Environmental Science and Technology, 2021, 51(8), 751. 15 Cui J, Liang S, Wang X, et al. Materials Chemistry and Physics, 2015, 161, 194. 16 Guo Y, Xia M, Zhang M, et al. Physical Chemistry Chemical Physics:PCCP, 2021, 23(11), 6632. 17 Zhu B, Zhang J, Jiang C, et al. Applied Catalysis B:Environmental, 2017, 207, 27. 18 Nie G, Li P, Liang J, et al. Journal of Theoretical and Computational Chemistry, 2017, 16(2), 1750013. 19 Gorai D K, Kundu T. Materials and Manufacturing Processes, 2020, 35(6), 625. 20 Gorai D K, Kundu T K. Materials Science Forum, 2020, 978, 369. 21 Gorai D K, Kundu T K. Materials Today Communications, 2021, 26(1), 101911. 22 Clark S J, Segall M D, Pickard C J, et al. Zeitschrift für Kristallographie-Crystalline Materials, 2005, 220(5-6), 567. 23 Perdew J P, Burke K, Ernzerhof M. Physical Review Letters, 1996, 77(18), 3865. 24 Tkatchenko A, Scheffler M. Physical Review Letters, 2009, 102(7), 73005. 25 Chadi D J. Physical Review B, 1977, 16(4), 1746. 26 Teter D M, Hemley R J. Science, 1996, 271(5245), 53. 27 Xie Z, Sui Y, Buckeridge J, et al. Applied Physics Letters, 2018, 112(26), 262101. 28 Wan J, Yang W J, Liu J Q, et al. Chinese Journal of Catalysis, 2022, 43(2), 485. 29 Ivanov A S, Miller E, Boldyrev A I, et al. The Journal of Physical Chemistry C, 2015, 119(21), 12008. 30 Zhu G, Lü K, Sun Q, et al. Computational Materials Science, 2014, 81, 275. 31 Li B, Nengzi L, Guo R, et al. Chinese Chemical Letters, 2020, 31(10), 2705. 32 Huang D, Wang K, Yu L, et al. ACS Energy Letters, 2018, 3(8), 1875. 33 Tang D, Zhong S P. Chemical Journal of Chinese Universities, 2021, 42(8), 2509 (in Chinese). 唐定, 衷水平. 高等学校化学学报, 2021, 42(8), 2509. 34 Guan Y Q, Hou Q Y, Gu Y L. Materials Reports, 2022, 36(2), 39 (in Chinese). 关玉琴, 侯清玉, 谷玉兰. 材料导报, 2022, 36(2), 39. 35 Zhang R, Xie D, Leng Y X, et al. Materials Reports, 2019, 33(Z2), 383 (in Chinese). 张然, 谢东, 冷永祥, 等. 材料导报, 2019, 33(Z2), 383. 36 Al F. Frontier Orbitals and Reaction Paths:Selected Papers of Kenichi Fukui, World Scientific, Japan, 1997, pp. 277. 37 Liu Z, Yu X, Li L. Chinese Journal of Catalysis, 2020, 41(4), 534. 38 Zhang L L, Xia T, Liu G A, et al. Acta Physica Sinica, 2019, 68(1), 245 (in Chinese). 张丽丽, 夏桐, 刘桂安, 等. 物理学报 , 2019, 68(1), 245. 39 Liu F Y, Xu L Y, Xiu Y, et al. Chemistry, 2021, 84(2), 108 (in Chinese). 刘方园, 徐鲁艺, 修阳, 等. 化学通报, 2021, 84(2), 108. 40 You X C. Journal of Chongqing University of Technology (Natural Science), 2020, 34(6), 123(in Chinese). 游晓畅. 重庆理工大学学报(自然科学), 2020, 34(6), 123. 41 Yan Y X, Zhang Y X, Zheng S, et al. Chinese Journal of Computational Physics, 2021, 38(4), 447 (in Chinese). 闫宇星, 张珏璇, 郑帅, 等. 计算物理, 2021, 38(4), 447. 42 Chen W, Meng Z S, Liang J W, et al. Science China:Physics, Mechanics & Astonomy, 2020, 50(4), 142 (in Chinese). 陈文, 蒙之森, 梁君武, 等. 中国科学:物理学 力学 天文学, 2020, 50(4), 142. 43 Pan F C, Lin X L, Cao Z J, et al. Acta Physica Sinica, 2019, 68(18), 141 (in Chinese). 潘凤春, 林雪玲, 曹志杰, 等. 物理学报, 2019, 68(18), 141. 44 Song X F, Sai X X, Li J, et al. Acta Physica Sinica, 2022, 71(1), 217 (in Chinese). 宋谢飞, 晒旭霞, 李洁, 等. 物理学报, 2022, 71(1), 217. 45 Fang W Y, Zhang P C, Zhao J. Materials Reports, 2021, 35(10), 10017 (in Chinese). 方文玉, 张鹏程, 赵军. 材料导报, 2021, 35(10), 10017. 46 Pham T A, Ping Y, Galli G. Nature Materials, 2017, 16(4), 401. 47 Sivasamy R, Paredes G K, Quero F. Physica E:Low-dimensional Systems & Nanostructures, 2022, 135, 114994.